Theoretical X-ray Absorption Spectroscopy of Liquid Water by the GW plus Bethe-Salpeter equation (GW-BSE) method

ORAL

Abstract

Oxygen K-edge x-ray absorption spectroscopy (XAS) provides an important local probe of the H-bond network in liquid water. Theoretical calculations of XAS spectra demand accurate modeling of both the molecular structure and the electron-hole excitation process. We generate the water structure from path-integral DeePMD calculations, whose neural network potential is trained on state-of-the-art DFT data at the SCAN0 hybrid functional level. Based on the above equilibrated trajectory, the XAS spectra of liquid water are computed by solving the Bethe-Salpeter equation (BSE) as implemented in the BerkeleyGW package. Our calculated XAS spectra of water agree well with experiments. Our results indicate that self-consistent GW quasiparticle wavefunctions and local-fields effects in electronic screening are crucial in the GW-BSE approach in order to yield XAS spectra that are in quantitative agreement with experiments.

*This work was primarily supported by the Computational Chemical Center: Chemistry in Solution and at Interfaces funded by the DoE under Award No. DE-SC0019394, and also supported by the Center for Computational Study of Excited-State Phenomena in Energy Materials (C2SEPEM) at the Lawrence Berkeley National Laboratory funded by the DOE under Contract No. DE-AC02-05CH11231.

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Presenters

  • Fujie Tang

    • Department of physics, Temple University

Authors

  • Fujie Tang

    • Department of physics, Temple University

  • Chunyi Zhang

    • Department of physics, Temple University
    • Temple University

  • Zhenglu Li

    • Department of Physics, University of California, Berkeley
    • UC Berkeley & Lawrence Berkeley National Laboratory
    • University of California at Berkeley, and Lawrence Berkeley National Laboratory
    • University of California at Berkeley and Lawrence Berkeley National Laboratory
    • Lawrence Berkeley National Laboratory
    • University of California, Berkeley
    • Lawrence Berkeley National Laboratory and University of California at Berkeley
    • Department of physics, University of California at Berkeley, Berkeley, California

  • Steven G Louie

    • University of California, Berkeley
    • Department of Physics, University of California, Berkeley
    • University of California at Berkeley and Lawrence Berkeley National Laboratory
    • UC Berkeley & Lawrence Berkeley National Laboratory
    • University of California at Berkeley, and Lawrence Berkeley National Laboratory
    • Lawrence Berkeley National Laboratory
    • Department of physics, University of California at Berkeley, Berkeley, California

  • Roberto Car

    • Department of Chemistry, Princeton University
    • Princeton University
    • Department of Chemistry, Princeton University, Princeton, NJ 08544, USA

  • Diana Qiu

    • Yale University
    • Department of Mechanical Engineering and Materials Science, Yale University
    • Mechanical Engineering and Materials Science, Yale University
    • School of Engineering and Applied Physics, Yale University

  • Xifan Wu

    • Department of physics, Temple University
    • Temple University